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Recycling
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Recycling of Spent Batteries—Trash to Treasure
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Recycling of Spent Batteries—Trash to Treasure

A special issue of Recycling (ISSN 2313-4321).

Deadline for manuscript submissions: closed (31 July 2023) | Viewed by 26585

Special Issue Editor

Dr. Anna Klemettinen

E-Mail Website
Guest Editor
Department of Chemical and Metallurgical Engineering, School of Chemical Engineering, Aalto University, 02150 Espoo, Finland
Interests: metallurgy; circular economy; metal recycling; battery metals; slag chemistry; phase equilibria

Special Issue Information

Dear Colleagues,

The demand for different types of batteries is expected to grow significantly in the near future. One of the major factors attributing to the increasing battery demand is the transportation sector, which is shifting towards lower emissions.

Spent batteries are a complex mixture of materials, and they require several different unit operations and processes to efficiently recover their components. Despite the enormous efforts made in recent years towards the development of new battery recycling technologies, the majority of spent batteries are still not being recycled. Moreover, many of the valuable battery components are lost in currently available recycling technologies.

Innovative recycling methods are needed to fulfill the rising demand for battery metals (e.g., lithium, cobalt, manganese, nickel) in order to meet the demands of green transitions in transportation as well as in many other sectors. Furthermore, the environmental impacts of battery recycling should be assessed as the environmental regulations are stringent.

We would like to invite colleagues to contribute their original research articles or reviews for this Special Issue on bringing value to spent batteries and closing loops in battery metal economy.

Dr. Anna Klemettinen
Guest Editor

Manuscript Submission Information

Manuscripts should be submitted online at www.mdpi.com by registering and logging in to this website. Once you are registered, click here to go to the submission form. Manuscripts can be submitted until the deadline. All submissions that pass pre-check are peer-reviewed. Accepted papers will be published continuously in the journal (as soon as accepted) and will be listed together on the special issue website. Research articles, review articles as well as short communications are invited. For planned papers, a title and short abstract (about 100 words) can be sent to the Editorial Office for announcement on this website.

Submitted manuscripts should not have been published previously, nor be under consideration for publication elsewhere (except conference proceedings papers). All manuscripts are thoroughly refereed through a single-blind peer-review process. A guide for authors and other relevant information for submission of manuscripts is available on the Instructions for Authors page. Recycling is an international peer-reviewed open access semimonthly journal published by MDPI.

Please visit the Instructions for Authors page before submitting a manuscript. The Article Processing Charge (APC) for publication in this open access journal is 1800 CHF (Swiss Francs). Submitted papers should be well formatted and use good English. Authors may use MDPI's English editing service prior to publication or during author revisions.

Keywords

  • metallurgy
  • recovery
  • lithium-ion battery
  • separation methods
  • critical raw materials
  • circular economy
  • environmental impacts

Published Papers (7 papers)

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Research

Jump to: Review

11 pages, 2726 KiB  
Article
Automated Battery Disassembly—Examination of the Product- and Process-Related Challenges for Automotive Traction Batteries
by Domenic Klohs, Christian Offermanns, Heiner Heimes and Achim Kampker
Recycling 2023, 8(6), 89; https://doi.org/10.3390/recycling8060089 - 08 Nov 2023
Viewed by 2656
Abstract
As the market share of electric vehicles continues to rise, the number of battery systems that are retired after their service life in the vehicle will also increase. This large growth in battery returns will also have a noticeable impact on processes such [...] Read more.
As the market share of electric vehicles continues to rise, the number of battery systems that are retired after their service life in the vehicle will also increase. This large growth in battery returns will also have a noticeable impact on processes such as battery disassembly. The purpose of this paper is, therefore, to examine the challenges of the battery disassembly process in relation to the required increase in the degree of automation. For this purpose, a survey of various experts along the battery value chain was conducted, and product-side hurdles, such as the wide range of variants, and process-side challenges, such as the opening of the housing cover or the removal of cables and connectors, were identified. Together with an assessment of the potential degree of automation in the context of downstream processes (reuse, repair, remanufacturing, and recycling), this results in a variety of streams for future research in the field of automated battery disassembly. The core aspect in this context is data availability consisting of product and component data as well as process-relevant parameters. Full article
(This article belongs to the Special Issue Recycling of Spent Batteries—Trash to Treasure)
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18 pages, 2457 KiB  
Article
Recovery of Graphite from Spent Lithium-Ion Batteries
by Charlotte Badenhorst, Iwona Kuzniarska-Biernacka, Alexandra Guedes, Elsayed Mousa, Violeta Ramos, Gavin Rollinson, Guozhu Ye and Bruno Valentim
Recycling 2023, 8(5), 79; https://doi.org/10.3390/recycling8050079 - 08 Oct 2023
Viewed by 2564
Abstract
Critical raw materials, such as graphite and lithium metal oxides (LMOs), with a high supply risk and high economic importance are present in spent lithium-ion batteries (LIBs). The recovery and recycling of these critical raw materials from LIBs will contribute to the circular [...] Read more.
Critical raw materials, such as graphite and lithium metal oxides (LMOs), with a high supply risk and high economic importance are present in spent lithium-ion batteries (LIBs). The recovery and recycling of these critical raw materials from LIBs will contribute to the circular economy model, reduce the environmental footprint associated with the mining of these materials, and lower their high supply risk. The main aim of this paper is to present a separation process to recover graphite from black mass (BM) from spent LIB. Simultaneously, LMO and copper (Cu) and aluminum (Al) foils were also recovered as by-products from the process. The process used a combination of simple and/or low environmental footprint technologies, such as sieving, sink-float, citric acid leaching, and milling through ultrasound and soft attrition, to allow separation of the LIB valuable components. Three graphite-rich products (with purities ranging between 74 and 88 wt.% total carbon and a combined yield of 14 wt.%) with three different sizes (<25 µm, <45 µm, and <75 µm), Cu and Al foil fragments, and an LMO-rich precipitate product are delivered. The developed process is simple, using low temperatures and weak acids, and using affordable and scalable equipment available in the market. Its advantage over other LIB recycling processes is that it can be implemented, so to speak, “in your backyard”. Full article
(This article belongs to the Special Issue Recycling of Spent Batteries—Trash to Treasure)
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Graphical abstract

19 pages, 26489 KiB  
Article
The Recycling of End-of-Life Lithium-Ion Batteries and the Phase Characterisation of Black Mass
by Laurance Donnelly, Duncan Pirrie, Matthew Power, Ian Corfe, Jukka Kuva, Sari Lukkari, Yann Lahaye, Xuan Liu, Quentin Dehaine, Ester M. Jolis and Alan Butcher
Recycling 2023, 8(4), 59; https://doi.org/10.3390/recycling8040059 - 12 Jul 2023
Cited by 1 | Viewed by 5137
Abstract
Black mass is the industry term applied to end-of-life (EoL) lithium-ion batteries that have been mechanically processed for potential use as a recycled material to recover the valuable metals present, including cobalt, lithium, manganese, nickel and copper. A significant challenge to the effective [...] Read more.
Black mass is the industry term applied to end-of-life (EoL) lithium-ion batteries that have been mechanically processed for potential use as a recycled material to recover the valuable metals present, including cobalt, lithium, manganese, nickel and copper. A significant challenge to the effective processing of black mass is the complexity of the feed material. Two samples of black mass from a European source were analysed using a combination of methods including automated SEM-EDS (AMICS) to characterise and quantify the phases present and particle chemistry. Micro X-CT imaging, overlain onto automated mineralogy images, enabled the 3D morphology of the particles to be determined. Micro-XRF was used to map the copper, nickel, manganese and cobalt-bearing phases. Since Li cannot be detected using SEM-EDS, its abundance was semi-quantified using laser ablation inductively coupled plasma mass spectrometry (LA-ICP-MS). The integration of these complimentary analytical methods allowed for detailed phase characterisation, which may guide the potential hydrometallurgical or pyrometallurgical recycling routes and chemical assaying. Full article
(This article belongs to the Special Issue Recycling of Spent Batteries—Trash to Treasure)
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14 pages, 2725 KiB  
Article
Kinetics of Zn–C Battery Leaching with Choline Chloride/Urea Natural Deep Eutectic Solvents
by Irlanda G. Cruz-Reyes, Jorge A. Mendoza-Pérez, Rosario Ruiz-Guerrero, Dulce Y. Medina-Velázquez, Luis G. Zepeda-Vallejo and Ángel de J. Morales-Ramírez
Recycling 2022, 7(6), 86; https://doi.org/10.3390/recycling7060086 - 18 Nov 2022
Cited by 2 | Viewed by 2534
Abstract
A choline chloride/urea natural deep eutectic solvent (ChCl NADES) was prepared via a green chemistry method and used to leach Zn and Mn oxides from conventional Zn–C scrap batteries. FTIR and 1H NMR spectroscopy were used to characterize the NADES. The leaching [...] Read more.
A choline chloride/urea natural deep eutectic solvent (ChCl NADES) was prepared via a green chemistry method and used to leach Zn and Mn oxides from conventional Zn–C scrap batteries. FTIR and 1H NMR spectroscopy were used to characterize the NADES. The leaching kinetics of the Zn and Mn oxides was monitored at isothermal conditions (80, 100, 125, and 150 °C) and at two solid/NADES ratios: 3.3 and 10 g dm−3. It was possible to dissolve Zn and Mn oxides under all of tested conditions, reaching more than a 95% recovery for both metals at 150 °C after 90 min, whereas, at 25 °C, it was possible to leach up to 90% of the Zn and 30% of the Mn after 4320 min (72 h). Furthermore, the leaching kinetics was controlled by the boundary layer, coincident with a shrinking core model. According to the Arrhenius plot, the activation energy for Zn ranges from 49.13 to 52.21 kJ mol−1, and that for Mn ranges from 46.97 to 66.77 kJ mol−1. Full article
(This article belongs to the Special Issue Recycling of Spent Batteries—Trash to Treasure)
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18 pages, 3586 KiB  
Article
Recycling of Lead Pastes from Spent Lead–Acid Batteries: Thermodynamic Constraints for Desulphurization
by Yongliang Xiong
Recycling 2022, 7(4), 45; https://doi.org/10.3390/recycling7040045 - 12 Jul 2022
Cited by 4 | Viewed by 3626
Abstract
Lead–acid batteries are important to modern society because of their wide usage and low cost. The primary source for production of new lead–acid batteries is from recycling spent lead–acid batteries. In spent lead–acid batteries, lead is primarily present as lead pastes. In lead [...] Read more.
Lead–acid batteries are important to modern society because of their wide usage and low cost. The primary source for production of new lead–acid batteries is from recycling spent lead–acid batteries. In spent lead–acid batteries, lead is primarily present as lead pastes. In lead pastes, the dominant component is lead sulfate (PbSO4, mineral name anglesite) and lead oxide sulfate (PbO•PbSO4, mineral name lanarkite), which accounts for more than 60% of lead pastes. In the recycling process for lead–acid batteries, the desulphurization of lead sulfate is the key part to the overall process. In this work, the thermodynamic constraints for desulphurization via the hydrometallurgical route for recycling lead pastes are presented. The thermodynamic constraints are established according to the thermodynamic model that is applicable and important to recycling of lead pastes via hydrometallurgical routes in high ionic strength solutions that are expected to be in industrial processes. The thermodynamic database is based on the Pitzer equations for calculations of activity coefficients of aqueous species. The desulphurization of lead sulfates represented by PbSO4 can be achieved through the following routes. (1) conversion to lead oxalate in oxalate-bearing solutions; (2) conversion to lead monoxide in alkaline solutions; and (3) conversion to lead carbonate in carbonate solutions. Among the above three routes, the conversion to lead oxalate is environmentally friendly and has a strong thermodynamic driving force. Oxalate-bearing solutions such as oxalic acid and potassium oxalate solutions will provide high activities of oxalate that are many orders of magnitude higher than those required for conversion of anglesite or lanarkite to lead oxalate, in accordance with the thermodynamic model established for the oxalate system. An additional advantage of the oxalate conversion route is that no additional reductant is needed to reduce lead dioxide to lead oxide or lead sulfate, as there is a strong thermodynamic force to convert lead dioxide directly to lead oxalate. As lanarkite is an important sulfate-bearing phase in lead pastes, this study evaluates the solubility constant for lanarkite regarding the following reaction, based on the solubility data, PbO•PbSO4 + 2H+ ⇌ 2Pb2+ + SO42− + H2O(l). Full article
(This article belongs to the Special Issue Recycling of Spent Batteries—Trash to Treasure)
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Review

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21 pages, 1946 KiB  
Review
Closing the Loop on LIB Waste: A Comparison of the Current Challenges and Opportunities for the U.S. and Australia towards a Sustainable Energy Future
by Gavin E. Collis, Qiang Dai, Joanne S. C. Loh, Albert Lipson, Linda Gaines, Yanyan Zhao and Jeffrey Spangenberger
Recycling 2023, 8(5), 78; https://doi.org/10.3390/recycling8050078 - 07 Oct 2023
Viewed by 3120
Abstract
Many countries have started their transition to a net-zero economy. Lithium-ion batteries (LIBs) play an ever-increasing role towards this transition as a rechargeable energy storage medium. Initially, LIBs were developed for consumer electronics and portable devices but have seen dramatic growth in their [...] Read more.
Many countries have started their transition to a net-zero economy. Lithium-ion batteries (LIBs) play an ever-increasing role towards this transition as a rechargeable energy storage medium. Initially, LIBs were developed for consumer electronics and portable devices but have seen dramatic growth in their use in electric vehicles (EVs) and via the gradual uptake in battery energy storage systems (BESSs) over the last decade. As such, critical metals (Li, Co, Ni, and Mn) and chemicals (polymers, electrolytes, Cu, Al, PVDF, LiPF6, LiBF4, and graphite) needed for LIBs are currently in great demand and are susceptible to global supply shortages. Dramatic increases in raw material prices, coupled with predicted exponential growth in global demand (e.g., United States graphite demand from 2022 7000 t to ~145,000 t), means that LIBs will not be sustainable if only sourced from raw materials. LIBs degrade over time. When their performance can no longer meet the requirement of their intended application (e.g., EVs in the 8–12 year range), opportunities exist to extract and recover battery materials for re-use in new batteries or to supply other industrial chemical sectors. This paper compares the challenges, barriers, opportunities, and successes of the United States of America and Australia as they transition to renewable energy storage and develop a battery supply chain to support a circular economy around LIBs. Full article
(This article belongs to the Special Issue Recycling of Spent Batteries—Trash to Treasure)
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17 pages, 688 KiB  
Review
The Application of Artificial Intelligence in the Effective Battery Life Cycle in the Closed Circular Economy Model—A Perspective
by Agnieszka Pregowska, Magdalena Osial and Weronika Urbańska
Recycling 2022, 7(6), 81; https://doi.org/10.3390/recycling7060081 - 07 Nov 2022
Cited by 8 | Viewed by 5988
Abstract
Global pollution of the environment is one of the most challenging environmental problems. Electronic-based population and anthropogenic activity are the main reasons for dramatically increasing the scale of waste generation, particularly battery waste. Improper battery waste disposal causes harmful environmental effects. Due to [...] Read more.
Global pollution of the environment is one of the most challenging environmental problems. Electronic-based population and anthropogenic activity are the main reasons for dramatically increasing the scale of waste generation, particularly battery waste. Improper battery waste disposal causes harmful environmental effects. Due to the release of heavy metals, battery waste affects ecosystems and health. We are faced with the challenge of effective battery waste management, especially recycling, to prevent the depletion of natural resources and maintain ecological balance. Artificial Intelligence (AI) is practically present in all areas of our lives. It enables the reduction of the costs associated with various types of research, increases automation, and accelerates productivity. This paper reviews the representative research progress of effective Artificial Intelligence-based battery waste management in the context of sustainable development, in particular, the analysis of current trends, algorithm accuracy, and data availability. Finally, the future lines of research and development directions of human-oriented Artificial Intelligence applications both in the battery production process and in battery waste management are discussed. Full article
(This article belongs to the Special Issue Recycling of Spent Batteries—Trash to Treasure)
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